A variety of complexes of the type Mo(NR) 2Cl 2L 2 (R = 4-Br-2,6- iPr 2-C 6H 2, 4-CN-2,6- iPr 2-C 6H 2, 3,5-Me 2- C 6H 3, 2- iPr-C 6H 4, 2-CF 3-C 6H 4, 2-Ph-C 6H 4, and 1-adamantyl; L = 1 2 DME or pyridine) have been synthesized by treating [NH 4] 2[Mo 2O 7]with four equivalents of RNH 2 in the presence of Me 3SiCl and Et 3N. They are readily alkylated by Grignard reagents to give complexes of the type Mo(NR) 2(CH 2R′) 2 (R = 4-Br-2,6- iPr 2-C 6H 2, 4-CN-2,6- i Pr 2-C 6H 2, 2,6-Me 2-C 6H 3, 3,5-Me 2-C 6H 3, 2- tBu-C 6H 4, 2- iPr-C 6H 4, 2-CF 3-C 6H 4, 2-Ph-C 6H 4, 1-adamantyl, R′ tBu or PhMe 2C) from which alkylidene complexes of the type Mo(NR)(CHR′)(OTf) 2(DME) are formed upon addition of triflic acid. Addition of various alkoxides to the triflate complexes yields four-coordinate complexes of the type Mo(NR)(CHR′)(OR″) 2 (combinations include R = 2,6- iPr 2-C 6H 3, 4-Br-2,6- iPr 2-C 6H 2, 4-CN-2,6- iPr 2- C 6H 2, 2,6-Me 2-C 6H 3, 3,5-Me 2-C 6H 3, 2- tBu-C 6H 4, 2- iPr-C 6H 4, 2-CF 3-C 6H 4, 2-Ph- C 6H 4, and 1-adamantyl; OR″ OCMe 3, OCEt 3, O-1-adamantyl, OCHMe 2, OCMe 2(CF 3), OCMe(CF 3) 2, OC(CF 3) 3, and OC(CF 3) 2CF 2CF 2CF 3).