We report the effect of carbon doping in Ti-stabilized nonstoichiometric molybdenum diboride (Mo 0.96 Ti 0.04 ) 0.8 B 2 , which exhibits bulk superconductivity below 𝑇 c = 7.0 K. It is found that (Mo 0.96 Ti 0.04 ) 0.8 (B 1−𝑥 C 𝑥 ) 2 maintains the AlB 2type phase with a uniform elemental distribution for 𝑥 = 0.12 and 0.16. The substitution of carbon for boron leads to a slight increase in 𝑎-axis, a remarkable reduction in 𝑐-axis, the formation of planar defects along the (100) crystallographic planes, and a shift of the B 1𝑠 peaks toward higher binding energies. Contrary to (Mo 0.96 Ti 0.04 ) 0.8 B 2 , however, no superconductivity is observed down to 1.8 K for the C-doped samples, which is ascribed to the electron filling of boron 𝜋 bands resulting from the carbon doping.