head to head
Neither is simply harder - they are hard in different places. Fallout 4 demands more variance; Portal 2 demands more optimization.

Optimization · Pure Optimization
An open-world shooter-RPG won by perk routing and weapon mod optimization.

Optimization · Pure Optimization
A first-person puzzle game where seeing the solution is the whole skill.
Fallout 4 leans Optimization (Pure Optimization); Portal 2 leans Optimization (Pure Optimization).
Fallout 4 leans a little harder on execution, though the gap is small.
Fallout 4
FPS aiming, VATS softens demand
Portal 2
Portal placement requires some precision but timing is lenient.
Fallout 4 leans a little harder on reads, though the gap is small.
Fallout 4
Scripted enemy AI
Portal 2
No opponent; puzzles are static.
Fallout 4 leans clearly harder on variance.
Fallout 4
Loot and legendary rolls
Portal 2
Puzzles are deterministic with no randomness.
Portal 2 leans clearly harder on optimization.
Fallout 4
Perks, settlement, weapon mod planning
Portal 2
Solving the puzzle's logic IS the entire game.
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.