The following rough approximation seems to show a neutron star at its Tolman–Oppenheimer–Volkoff limit of 2.17 solar masses and 12km radius, has gravitational binding energy on the same order as its relativistic mass-energy:
$$\frac{3}{5} \frac{(2.17*1.989*10^{30}kg)^2G}{12km}=6.2*10^{48}J$$ $$2.17∗1.989∗10^{30}kg *c^2=3.88*10^{48}J$$
While numbers and formula I've used are very rough -- which would explain the apparent 60% excess -- it does seem as though once a TOV star has settled down through radiation, just about all of its mass has been effectively converted to energy. Is this correct? If not, how much of its primordial (H, He, etc.) mass has been converted to energy?