Propagation of few-cycle optical pulses in nonlinear optical Kerr (cubic) and non-Kerr (quintic) type metamaterials, exhibiting frequency-dependent dielectric susceptibility and magnetic permeability, is considered. Considering the theory of electromagnetic waves from Maxwell’s equations, a new nonlinear evolution equation describing the combined influences of higher-order nonlinearities and higher-order linear and nonlinear dispersions, appropriate for electromagnetic ultrashort pulse propagation in negative index materials, is derived beyond the slowly varying envelope approximation. A fully numerical simulation of the newly derived model equation, based on the lossy Drude model, shows the propagation of soliton-like stable few-cycle optical pulses under some parameter values. The change in types of self-steepening parameters induces structural changes of the initial input pulse, characterized by a soliton molecule made of either asymmetric or symmetric optical pulses. Also, the mutual balancing between Kerr and non-Kerr nonlinearities and higher-order dispersions is found to support the formation of soliton-molecules in both the normal and anomalous group velocity dispersion regimes.