Measurements have been made of the spin-lattice relaxation times of 51V nuclei in alloys across the V-Cr system. The product of relaxation time and temperature is independent of temperature but strongly dependent upon composition, increasing monotonically from 0.795 sec °K in pure V to 8.48 sec °K in V-90 at.% Cr. This composition dependence is compared with that of the electronic specific heat of V-Cr alloys. It is concluded that a valid description of the V-Cr system is given by a simple theoretical model containing separate 3d and 4s bands. The contribution to relaxation from the 4s band is only about 3% of the total in pure V but provides about 40% at the Cr-rich end of the system. The main 3d contribution is through orbital or core-polarization interactions, or a combination of these. The two-band model is found to be consistent with the behaviour of the magnetic susceptibility and nuclear resonance shift in these alloys. Magnitudes are derived for the various contributions to these two properties. Of the total paramagnetism of pure V, about 2% is due to 4s spin paramagnetism, about 50% is orbital paramagnetism and the remainder is due to 3d spin paramagnetism. At the Cr-rich end, the corresponding contributions are respectively about 3%, 75% and 20%. Of the nuclear shift in pure V of 0.58%, 0.045% is from the 4s band, between 0.54% and 0.82% from the orbital paramagnetism of the 3d band and the remainder is made up by a diamagnetic contribution from core polarization. The corresponding figures at the Cr-rich end of the system, where the total shift is 0.54%, are 0.045%, about 0.58% and 0 to -0.06%.