Current interests in the chemistry of the early actinide elements are divided into two categories; (1) high valent actinyl ions, principally uranyl(VI), which display the rich combination of coordination ability and photo-redox activity, and (2) low valent ions, predominantly uranium and thorium(III and IV), complexed by ancillary ligands designed for organometallic applications. The structural, photo-, and electrochemical properties of a diverse series of uranyl(VI) schiff base complexes will be presented, and in one instance the photolysis of UO₂SalophenTHF in the presence of cobaltocene and tetrahydrofuran direct an unconventional reactive luminescent pathway. Also, the photochemical reduction of a well defined uranyl chloride material has proven to be a convenient synthetic route to access a monomeric uranium(IV)-trichloride supported by triphenylphosphineoxide and alkoxide ancillaries.