Anyone know why?
No idea about your issue, but...
Why have you bothered enchanting stuff with Fortify Lockpicking? Seriously, that is a waste of soul gems.
My friend I'm sorry but I will give you a break down of what's happening...
1. You're game has been possessed by the Daedric lord Sanguine and he is pranking you hardcoe this could cause an actual demonic force to enter the game and you will have a similar experience like 'What happened to Bill' or 'Lavender Town effect'
2. You're character and game is growing a mind of it's own and has gained a conscience and has decided it doesn't want to adventure, do anything dangerous, or illegal and has no intention of helping you again sorry but kiss your dreams of being a master thief goodbye
3. Or finally there's a glitch in the Matrix and you know to much and must be 'put to better use' prepare to be assimilated!
Beats me but why not travel to a shrine or temple and get a god's blessing to make sure. Also check Active Effects.
The higher you lockpicking skill, the harder the lock will be to pick. I have never heard of this before, and I have no problems. Just take your time, for you are probably missing the "sweet spot."
There was a bug where lockpicking over 100 would make picking impossible, but it was fixed in official patch 1.3. You do have the update esm or PS/Xbox patch installed?
I seem to remember, not specific to lockpicking, but sometimes if you have too much gear that boosts a given skill, it can kinda cause things to go kerflooey. Have you tried picking a lock without your lockpicking gear?