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I don't know what number would be good, but you might have to increase it quite a bit.
Base success rate is something like Enchant Skill + (Int/5) + (Luck/10) - Spell Difficulty
So if you have 100 Enchant, 100 Int, and 100 Luck, it would look something like... 160% - Spell Difficulty, which depends on what you're trying to enchant.
Spell Difficulty depends on the potency of the spell you're trying to enchant. I don't know the exact numbers.
The Morrowind Code Patch should have something that lets you see your actual success rate before you enchant, though. At least in one of its more recent updates.
You can modify the skill progression so each success adds loads to the bar, even a whole level or more. You can adjust the volume of soul gems, size of souls, capacity of items and cost of enchantments. You can also change which magic effects are enchantable. You can do all of these to make Enchant more user friendly and not feel you have to max out enchantments to get anything worthwhile.
You cannot modify the chance for success. That seems to be hard coded or just so well hidden nobody has found it in 15 years. It's not under the Enchant skill entry nor the spell effect menus.
You can use god mode...
From the UESP wiki:
The percentage chance to successfully self-enchant an item is:
- Enchant Skill + [Intelligence/4] + [Luck/8] - [ 2.5x Enchant Value for Cast When Used/Strikes, or 5x Enchant Value for Constant Effect]
Where Enchant value refers to the amount of points used by the enchantment, not the maximum enchantment points the item can hold.
To put this into perspective: Say you have a character with 40 Luck and 60 Intelligence [typical starting stats for a Mage]. To make yourself an item with only 1 Enchant Value at 100% chance [which is not very much at all, maybe a Restore Fatigue 39 points spell], requires your character to have enough Enchant skill to get that formula to 100%. 40/8 = 5% from luck, 60/4 = 15% from Intelligence, and 1x2.5 = -2.5% from the 1 Enchant Value. That's 17.5% success rate without counting Enchant skill.
Which means that, for even as crappy an item as the one described above, to have a 100% success chance of making it with the above character, requires 83 ENCHANT SKILL. And this is only a crappy Cast When Used item.
In other words, you'll want to Fortify your Enchant skill a LOT if you want to make any decent items yourself with it. From memory, in order to make a super-powerful Constant Effect enchantment on the best 'Enchant Value' item in the game [Daedric Tower Shield, 225 possible Enchant Value], you need something like 1200 Enchant skill. Which is impossible to attain without Fortifying it, so you're going to want some option to Fortify either your Skill or Intelligence.
If you have the Expansion Packs, a Fortify Skill spell is available from within the palace of Mournhold off of one of the spell merchants [i.e. where you get teleported to start with from Ebonheart]. If you can grab one of these, and then PAY SOMEONE for a Fortify Enchant 100 points for 1 sec on self Cast When Used Item [or make it into a Restoration spell that you can cast], then you can use that to make other items, including further Fortify Enchant skill items. Paying for small Enchanted items early on is not too expensive; a few thousand gold at most [which can be found or procured from loot and/or various quest lines].
Just remember that in order to make a 1 second Enchantment, you have to FIRST increase the Duration up a bit, and then decrease it back down to 1. Else the spell will be instant and you won't be able to use it on yourself effectively.
If you have some Alchemy skill and the right ingredients [Ash Yams and Bloat, like psychotron suggested], Fortify Intelligence potions are another option. You can use these to make even better Fortify Intelligence potions, such that potion strength becomes gamebreakinig [i.e. 10,000+ points of Fortification]. You may want to avoid this method or sleep through the potion Duration if you're a little worried about being so broken outside of just making items, especially given that you're a mage.
In the mean time: what levelling Enchant between 0-100 IS useful for, is conserving Charge when using items. The difference between using an item with 5 Enchant skill vs at 100 Enchant skill is about 10x the difference [e.g. an Amulet of Recall at 5 Enchant uses 18 Charge, and at 100 Enchant uses 2 Charge]. Not only that, if you increase it to at least 110, every item [even stupidly powerful ones] will only cost 1 charge to use. The skill levels reaaaalllyyy slowly however, so it's more beneficial to buy training than to try and increase it naturally.
tl;dr Find a Fortify Skill/Intelligence option if you want to make items yourself, and then purchase some training [Ajira in Balmora, Skink in Tree's Shade in Sadrith Mora, Quorwyn in Indoranyon if you're crafty and have a Calm Humanoid spell]] to get your charge cost down.
I had a 35 enchant skill fortified int to 90 and luck to 50 and made a belt that fotifies luck/int to 100 with a lesser soul gem with a summoned skelington soul in it. So now I can do what I wish in terms of enchanting