head to head
Neither is simply harder - they are hard in different places. Portal 2 demands more optimization; The Legend of Zelda: Twilight Princess demands more variance.

Optimization · Pure Optimization
A first-person puzzle game where seeing the solution is the whole skill.

Optimization · Pure Optimization
Darker cinematic Zelda alternating wolf form and classic dungeon crawling.
Portal 2 leans Optimization (Pure Optimization); The Legend of Zelda: Twilight Princess leans Optimization (Pure Optimization).
The Legend of Zelda: Twilight Princess leans a little harder on execution, though the gap is small.
Portal 2
Portal placement requires some precision but timing is lenient.
The Legend of Zelda: Twilight Princess
Hidden sword skills add modest combat depth
Same score on reads - which means the number cannot separate them. The difference is in what each one asks of you.
Portal 2
No opponent; puzzles are static.
The Legend of Zelda: Twilight Princess
Scripted bosses and enemies
The Legend of Zelda: Twilight Princess leans clearly harder on variance.
Portal 2
Puzzles are deterministic with no randomness.
The Legend of Zelda: Twilight Princess
First-run exploration unknowns
Portal 2 leans clearly harder on optimization.
Portal 2
Solving the puzzle's logic IS the entire game.
The Legend of Zelda: Twilight Princess
Dungeon-item puzzle chains and wolf-form routing
A matching score does not mean a matching test. Two games can both sit at 10 on execution and demand completely different things of you - which is why the reasoning above matters more than the number beside it.