The new ternary pnictides, Ti(1-delta)Mo(1+delta)Pn(4) (Pn = As, Sb), were uncovered during our search for novel thermoelectric materials. Both compounds crystallize in the OsGe2 type in the monoclinic space group C2/m, with lattice dimensions of a = 10.1222(9) A, b = 3.6080(3) A, c = 8.1884(8) A, beta = 120.230(2)degrees, and V = 258.38(7) A(3) (Z = 2) for Ti0.79(1)Mo1.21Sb4 and a = 9.1580(2) A, b = 3.3172(1) A, c = 7.6666(1) A, beta = 119.496(1)degrees, and V = 202.720(4) A(3) (Z = 2) for Ti0.86(2)Mo1.14As4. The electronic structure calculations predicted metallic behavior for these compounds, which was in agreement with the measured temperature dependence of the electrical conductivity and Seebeck coefficient.