This paper focuses on Hybrid Energy Storage Systems (HESS), consisting of a combination of batteries and Electric Double Layer Capacitors (EDLC), for electric urban busses. The aim of the paper is to develop a methodology to determine the hybridization percentage that allows the electric bus to work with the highest efficiency while reducing battery aging, depending on the chosen topology, control strategy, and driving cycle. Three power electronic topologies are qualitatively analyzed based on different criteria, with the topology selected as the favorite being analyzed in detail. The whole system under study is comprised of the following elements: a battery pack (LiFePO4 batteries), an EDLC pack, up to two DC-DC converters (depending on the topology), and an equivalent load, which behaves as an electric bus drive (including motion resistances and inertia). Mathematical models for the battery, EDLCs, DC-DC converter, and the vehicle itself are developed for this analysis. The methodology presented in this work, as the main scientific contribution, considers performance variation (energy efficiency and battery aging) and hybridization percentage (ratio between batteries and EDLCs, defined in terms of mass), using a power load profile based on standard driving cycles. The results state that there is a hybridization percentage that increases energy efficiency and reduces battery aging, maximizing the economic benefits of the vehicle, for every combination of topology, type of storage device, control strategy, and driving cycle.