I think you misunderstood the parent comment. They're not talking about defining the reals by setting up a mapping where each real number corresponds to a unique natural number. They're talking about defining the reals by setting up a mapping where each real number corresponds to a unique mapping from the natural numbers to {0, 1} (i.e. a unique binary sequence). The set of all binary sequences is isomorphic to the power set of the natural numbers, which is uncountable.

I'm not a set-theorist, but a set-theorist friend of mine once taught me that you can turn a countably-infinite set (such as the integers) into an uncountably-infinite one (like the reals) by applying the 'power set' operation (the set of all subsets).

Not heaps sure what this really means with respect to whether 1 the integer is really completely related (as in, equal, or the-exact same-thing) to 1.0 the real though. Kinda seems like it might still need a bit more information to fully identify a real, even when it happens to be infinitely-close to an integer?

You can't map the natural numbers to the set of real numbers, but you can map the natural numbers to the fractional part of a single real number.

Fortunately functions from the natural numbers are not countable either. This is Cantor's theorem.