In elemental metals the pairing of electrons leading to superconductivity is mediated by the vibrations of the crystal lattice and the pairs have spherical symmetry. For layered organic molecular crystals there is no consensus about the pairing symmetry or the mechanism of the superconductivity. We show theoretically that the mechanism of superconductivity for members of the (BEDT-TTF)2X family with the theta and beta'' crystal structures is mediated by charge fluctuations and the superconducting order parameter has dxy symmetry. This is in contrast to the kappa-(BEDT-TTF)2X family, for which theoretical calculations give superconductivity mediated by spin fluctuations and with dx2-y2 symmetry. Our conclusions are based on systematic many-body calculations using slave-boson theory of an extended Hubbard model. This is the simplest model that can describe the competition between metallic, superconducting, insulating, and charge ordered phases that occurs in the theta and beta'' materials. Based on the theory presented we predict several materials that should become superconducting under pressure.