Yes, as Bad-People said, it works best with all 4.
Gather yourself 4 full grand soul gems, and make or acquire a ring, necklace, gloves or bracers, and a helmet or circlet. Hands, finger, neck, head. Also, get hold of an Enchanter's Elixir if you can. That seems to be the strongest. Skyrim time does not seem to mirror real time, and I have found 30 seconds to be considerably shorter, so don't waste any time on the enchanter with naming them or anything.
I would go to the enchanter with nothing else non-magical on, so there are not extra choices in the enchant menu. Disenchant your bracers and learn the secret first, before you drink the potion. Then quit, drink, return, and quickly enchant all four items while you have the bonus. If you think you may be slower, then try to get two Elixirs and do it two at a time.
Once you've done that, return to your alchemy lab in all four garments (again, with nothing else extra to clog up your menu choices, so put all armor and apparel, as well as all potions and non-necessary ingredients away.)
At a minimum, keep your abs. longfin and cyrodillic spadetail, some salt piles, and if you have them any small pearls or small antlers. One of each, plus a salt pile, will make your restoration potions...no need to waste other ingredients. Always couple them with salt pile, because it's more easily obtained and cheaper.
Take a count of how many potions you can make. Let's say you have enough material for 10 potions. I would recommend doing this only 8 times (the make, drink, unequip, re-equip, etc.) and then use the last two sets of materials to make two potions at the top end. If you want to really overpower your weapons and armor, add some blisterwort, glowing mushroom, spriggan sap, and sabre cat tooth to your inventory before you start. Here again, it only takes two ingredients to make the potion.
Lock yourself into a quiet alchemy lab, make your follower wait somewhere they can't talk to you, and you're ready to start. Equip your lab apparel, make the first potion, quit, unequip, drink, close and reopen menu, re-equip and go again. Remember to save two potions worth. When you reach that point, make what will be your most-powerful potion twice, then immediately make as many fortify smithing potions as you can. If you have another pet potion, this is the time to crank out as many as possible but this also adds more potentially confusing choices to your menu.
Once you're all done, you should have two very powerful restoration potions and however many very powerful smithing potions. You want to do the same thing with smithing enchantments, always using grand soul gems, only it's ring, necklace, bracers and armor or clothes rather than headwear. When you go to smith up, take only what you want to upgrade (it doesn't work at the forge, only stone and bench). Make certain you have enough of and the right kind of ingots to do the upgrade, and again make the follower wait somewhere else.
If you're doing this in whiterun, do it after hours so whatshername can't get in your way. For this, you don't need to unequip and re-equip. Just go to the stone, make sure your enchanted apparel is equipped, drink a smithing potion immediately followed by a restoration potion (the enchanted clothes are restoration magic). Quickly upsmith your weapons first, then jump to the bench and do your armor. (armor has a cap of I think 567...weapons do not....strong offense and all that...) You should come away with some kickass armor, a few potions in case you want to do it again, and a spare restoration potion from which you can start your build the next time. Good luck.
