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Data on the ways of controlling the molecular structure of polyethylene (PE) synthesized over the supported catalysts containing Fe(II) bis(imino)pyridyl (LFeCl2) and Ni(II) bis(imine) (*LNiBr2) complexes immobilized on a silica gel modified with aluminum oxide (SiO2(Al)) are presented. Linear polyethylene with different molecular masses and a controllable molecular weight distribution (MWD) is synthesized by varying the conditions of polymerization on LFeCl2/SiO2(Al) catalysts. Ethylene homopolymerization over *LNiBr2/SiO2(Al) catalysts results in branched polyethylene with molecular mass and thermophysical characteristics close to that of low density polyethylene synthesized by ethylene copolymerization with α-olefins over supported metallocene and Ziegler type catalysts. A way for designing supported bicomponent catalysts containing LFeCl2 and *LNiBr2 complexes immobilized on an SiO2(Al) support for the targeted synthesis of polyethylene with a required molecular structure is proposed. Examples are given for the synthesis of linear polyethylene with a bimodal MWD on a bicomponent supported catalyst containing two different LFeCl2 complexes, the synthesis of polyethylene with a controllable distribution of branches on a bicomponent catalyst prepared via the immobilization of LFeCl2 and *LNiBr2 complexes on a SiO2(Al) support, and the modification of a chromium oxide catalyst with LFeCl2 complex for controlling the molecular mass and branch distributions in synthesized polyethylene are given. [ABSTRACT FROM AUTHOR]