I'm not a chemist but are there really no alternatives? Running fusion plants to make helium seems very unlikely to become cost effective, but it would be quite the sci-fi future if we filled party balloons by bombarding hydrogen with free protons.
I guess there aren't any easy molecules to break apart to get helium either since its a noble gas. No hydrolyses type solutions because there aren't any molecules that incorporate helium. I guess radioactive decay, but even that is ultimately limited over long enough timescales.