AbstractThe electron projection functionP(x,z) = ∫ ρ(x,y,z)dyis used to evaluate charge transfer and covalency in two series of molecules, LiX and CH3X (X = Li, BeH, BH2, CH3, NH2, OH, and F), with wavefunctions derived from STO‐3G, 4‐31G, and, in some cases, 6‐31*ab initiocalculations. The precision of the method and comparison with Mulliken populations analysis are described. Particular attention is given to CH3Li which by our criteria is whol