Compounds of the general type (η5-C6H4R)M(CO)2NO have been prepared and their chemistry has been studied, where M = Cr, Mo, and W and R = C02CH3, CHO, COCH3, C(CH3)=CH2, and CH[N(CH3)2]CH3. The carbomethoxy derivatives (R = C02CH3) for all three metals (M = Cr, Mo, W) were obtained in yields of 12-79%. The acetyl (R = COCH3) and formyl (R = CHO) derivatives were obtained only for M = Cr in yields of 79% and 56%, respectively. The isopropenyl organometallic monomers (R = C(CH3)=CH2) have been prepared for molybdenum and tungsten in good yields. Treatment of 6-(dimethylamino)fulvene with methyllithium followed by molybdenum hexacarbonyl and subsequent nitrosylation with N-methyl-N-nitroso-p-toluenesulfonamide gave the (dimethylamino)ethyl derivative (R = CH[N(CH3)2]CH3; M = Mo) in 56% yield. A reaction between lithium nitrocyclopentadienide and chromium hexacarbonyl followed by acetic acid and -Nmethyl-N-nitroso-p-toluenesulfonamide gave the reduced compound (η5-C6H4NH2)Cr(CO)2NO in 7% yield.