He has never activated Limiter Removal. He had it in his hand once, against Jaden. That's it. If I had to name a "signature spell" of his, it'd be Vehicroid Connection Zone, there's really no other choice.
Heck even Ruka/Luna from 5Ds used Limiter Removal once when she used her brother's deck.
Syrus on the other hand, only has it in his hand once, and never use it.
It's clearly not his signature Spell card.
I think you mistook Limiter Removal with Power Bond, another ATK-doubling Spell card for Machines that Syrus was afraid to use at first.
I think that if they put power bond and limiter removal in game everyone will go for machine decks. If they want to put power bond or limiter removal, they should choose one, otherwise it will be overpowered.