Make the triangular fold at the centre corner a 45° fold — that is, fold so that the crease cuts off equal lengths along the two edges meeting at the centre.
Cut off length d on each of the two perpendicular creases
The four crease segments each measure √(d² + d²) = d√2 ⇒ all sides equal
The diagonals of the figure are both 2d ⇒ equal diagonals
They bisect each other at 90° (the original two folds)
⇒ equal diagonals, bisecting each other at 90° ⇒ a square
The easiest way to be exact: bring one of the two creases exactly onto the other at the centre corner. That fold bisects the right angle, so it makes 45° with each — and it automatically cuts off equal lengths.
Why unequal cuts fail: if you cut off d along one crease and a different length e along the other, the diagonals become 2d and 2e. They still bisect each other at 90°, so you still get a rhombus, but unequal diagonals mean unequal — not right — angles. Only d = e makes the diagonals equal, and only then is the rhombus a square.