Libra pondo means “weighing a libra,” and yes, it is redundant. We can see this because while we can see Romans writing things like:
- argenti decem pondo libras habere (A. Gellius)
- libram pondo aeris valere (Varro)
⋯ we also see many cases where they only say libra or only pondo:
- libra ocellatorum (Varro; an ocellatum is apparently some kind of gem or die)
- corona aurea librarum quinque (Suetonius)
- auri quinque pondo (Cicero)
- argenti pondo viginti millia (Caesar)
Let us look at the words individually:
libra is the name of a Roman unit of weight, which is around 326 g (estimations for the exact value vary a few grams up and down). It is usually translated as “pound” (as are Romance words derived from it, e.g. French livre). It does not mean “weight” per se, but it generally unequivocally refers to a weight, so we do not necessarily have to specify that we are talking about weight.
pondo is not, as Wikipedia says, simply “the ablative singular of the Latin noun pondus,” because that would be pondere. It is indeed understood as stemming from an ablative singular, but it is usually parsed as an adverb meaning “weighing, by weight.” As such, in principle, it has to go along with some quantity, e.g. libra pondo.
However, if no unit is specified, it works as an undeclinable noun meaning pound or pounds. In effect, when a Roman says “gold weighing five” (auri quinque pondo), he means “five pounds of gold” (circa 1.6 kg). And this was a very common way to talk about weights. The English term “pound” (and others, e.g. German „Pfund“) are derived from it.
The way you phrased your question – isn't libra pondo pleonastic – suggests you are surprised the Romans would have used a redundant expression. But redundancy is very common throughout human speech. After all, “a bag weighing 5 kg” is also redundant, as the kilogram is a unit of weight, and it would suffice to say “a bag of 5 kg.”