The preparation of dialkyl-aluminium, -gallium, and -indium cyclopentadienyls, R 2MCp, is described. For the diethyl derivatives, a detailed analysis of the IR and Raman spectra in both solid and liquid phase clearly rules out a σ-bonded structure. pentahapto ( h 5) Cyclopentadiene—metal bonding can be established for the diethylalumiuium cyclopentadienyl ether adduct; for the uncomplexed compounds, spectral evidence points towards h 2/ h 3 bonding.