I'm somewhat new to modding and am having difficulty figuring out how to do this. I would like to establish a hard cap to armor/weapon quality to the initial 'legendary' tier in an effort to balance weapon and armor types against one another. Can anyone point me in the right direction on how I might accomplish this?

ASBE (Alek's Skyrim Balance Experience) on skyrimnexus removes all potion effects that boost smithing and enchanting, that helps.
You could similarly change the smithing enchantment effect to do something else entirely, or simply remove all items which have such enchantments (except for the Forgemasters Fingers; just make that unable to be disenchanted.)

To do what you are asking directly you would probably need to have a script and I am useless at scripting, so I'll stop now.

Thanks, but it sounds like that mod is no different from a conscious choice not to use potions for smithing and/or enchanting. What I'm looking for is a hard cap that allows weapons and armor, to all reach the same tier of 'legendary' quality, whether they have a smithing perk associated with them or not. This would allow for more varied gameplay as it would result in Light Armor having a very real difference from Heavy Armor as well as Daedric artifacts maintaining an edge against similar, crafted weapons and armor.