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Otherwise, info on where to loot!
https://fallout.fandom.com/wiki/Concrete_(Fallout_4)
Vault 114 is an okay source because there are a dozen cement bags, but you'll need companions or Strong Back because they'll weigh 75045204 pounds
one single command: player.additem 1ec66a 100, gives you 100 of those shipment certificates Chaos is talking about, except without buying one, sleeping for 3 days til they restock or speeding up the regen with a console command, and buying 1 more... this will give you 100 of *EVERY* certificate, all possible components, and of course they weigh nothing so when you craft with them, the remainder of the heavy supplies go into the workbench.
Is it cheating? no. yes. maybe? who cares, exactly? it's a single player game.
if you're ok with it, we're ok with it.
The most concrete I always get from totally scrapping Sanctuary. I never do the Minutemen quest (or any other major questlines), so Sanctuary is empty anyway and is only a point for a caravan connection.
Then there are more than usual concrete blocks found in Taffington boathouse, you also don't need to do a quest to get access to the workbench there, just kill the bugs.
Other than that, as said, buying shipments is the only way for getting bigger numbers.
https://www.nexusmods.com/fallout4/mods/4649
Also I'd suggest one that's at least configurable, and supports a bunch of mod-provided vendors too, very few gamers are running vanilla this many years down the line...
https://www.nexusmods.com/fallout4/mods/64017
y'know you can always 'tcl' and look behind the walls/floor and find the nearby vendor container and manually reset it as you want, but yeah, that's not any more immersive than just giving yourself the certificates, so nevermind.
Son of a........ I've been using a batch file with all the material IDs... Spawning an absolute obscene amount of junk into my inventory and having to dump it at a workbench...
It absolutely is, but who gives a damn...? I've spent many many many hours building things in this game before. If I'm starting a new play through, I'm going to take a couple of shortcuts to skip the boring bits...
Time is a valuable thing in life and some people don't have enough of it.
https://falloutcheats.com/items/material
It's not my personal method, but it's certainly convenient.
This is the best legitimate answer if you want to make massive concrete works in your settlements.