The reaction between TMSN3 and [Mo(TPP)]2 or Mo(TMP) proceeds in a refluxing alpha-chloronaphthalene medium to produce these red-purple solid compounds. N=Mo(TMP), further characterized by single crystal X-ray diffraction, crystallized in the space group P1BAR (No. 2) with a = 12.019(86) angstrom, b = 16.781(61) angstrom, c = 13.412(76) angstrom, alpha = 93.164-(3)degrees, beta = 99.539(3)degrees, gamma = 99.360(3)degrees, V = 2622.9 angstrom3, Z = 2, and rho(c) = 1.145 g-cm-3. Data in the range 2-degrees < theta < 50-degrees were collected, yielding 9623 unique reflections. The final discrepancy indices were R = 6.1% and R(w) = 7.1% for the 7576 reflections with I > 2sigma(I) used for structure solution employing least-squares refinement of 559 parameters.