An aspect of the invention relates to a method of synthesizing a crystalline molecular sieve having an MSE framework type, the method comprising crystallizing a reaction mixture comprising a source of water, a source of an oxide of a tetravalent element, Y, selected from at least one of silicon, tin, titanium, vanadium, and germanium, optionally but preferably a source of a trivalent element, X, a source of an alkali or alkaline earth metal, M, a source of a first single-nitrogen-containing cyclic ammonium organic cation, Q1, and optionally a source of a second multiple-nitrogen-containing organic cation, Q2, which can include multiple-nitrogen-containing monocations and/or multiply ionic species containing two or more ammonium cations in the same molecule.