We can, but not enough to justify the cost. We can even convert the alpha/beta radiation into electricity directly, but the conversion efficiency is extremely poor so you’d need a high activity (dangerous) source that likely won’t be around for very long (short half life).
Someone from a nuclear waste disposal organisation I visited was asked the question “what would happen if you put a spent fuel cask in your basement”. She said, “you won’t have to pay for heating for the next few decades, but in return the [country’s nuclear regulator] and police will be paying regular visits to your house to check that nothing has gone missing and everything is still stored properly”.
So spent fuel is pretty efficient as a space heater – but you can’t just give the stuff out for safety and proliferation reasons.
TLDR: you can, it’s just not economical.
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