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Abstract: Polyethyleneimine molecules alkylated with naphthylmethyl bromide and benzyl bromide and internally cross-linked by reaction with alkyl dihalides have binding capabilities enhanced by up to twofold. The modified and cross-linked polyethyleneimines bind large numbers of methyl orange dye molecules; since no evidence is found for dye stacking the cross-linked polyethyleneimine is considered to retain the flexibility of the native material. Increasing the cross- linking percentage from 0 to 20% of the available nitrogen causes a modest twofold increase in binding strength; cross- linking of polyethyleneimine in the presence of methyl orange dye produces a polymer which has doubled binding capacity for this dye than has the polymer cross-linked in the absence of added dye. Cross-linking does not reduce the number of primary amines in the alkylated polyethyleneimine available for reaction with Cu (1) ions or with 2,4,6- trinitrobenzenesulphonate anion. The reactivity of the cross- linked polymers with 4-nitrophenyl esters is not reduced below that of the native polyethyleneimine