abundant renewable energy source, the solar-rechargeable electric energy storage systems (SEESSs), which convert solar radiation to electricity via the PV components while the complementary ESSs directly store the as-generated electrical energy, is one of the most promising nextgeneration power sources. [5][6][7] Considerable research efforts have been devoted to the development of high-performance SEESSs to meet the diverse energy demands, which require both high power density and high energy density. [4,8] However, the state-of-the-art SEESSs consisting of photovoltaics and lithium-ion batteries (LIBs) have fundamental limitations such as low power density (Scheme 1a) and poor energy storage efficiency (ESE) under high charge-discharge rate because of the limited rate performance of LIBs. [4,5] For example, the energy density and ESE of a LIB only retain less than 50% and 60% of its original values when the current density increases from 85 to 850 mA g −1 . [9] To address these issues, much effort has been made to exploring combination of PVs with supercapacitors (SCs), which show excellent power density. [10][11][12] Nonetheless, the PVs-SCs systems still face a number of challenges including the low operation voltage (mostly below 0.8 V), and more critically, limited energy density (usually lower than 15 Wh kg −1 , Scheme 1a). [13,14] The emerging aluminum ion batteries (AIBs) showing fast chargedischarge feature provide a new avenue to achieve both high power density and large energy density, leading to constantly high ESE under ultrahigh charge-discharge rates. [15] Other important merits such as abundant Al resources, increased safety, and long cycling stability together make AIBs promising energy storage candidates for portable SEESSs, but their use for next-generation SEESSs has yet been reported. [16][17][18][19] In addition to the improvement of energy storage part, optimized modulation is also urgently required for the portable SEESSs, to achieve higher overall photoelectric conversion and storage efficiency (PCSE). [20] One major obstacle in achieving efficient solar-charging is the incompatible current-voltage characteristics between multi-junction PVs and ESSs. [21] The mismatch between the maximum power point (MPP) of PV and charge voltage of ESS results in significantly reduced solar to battery charging efficiency and thus a lower overall PCSE. [11] Furthermore, the external electrical circuit connecting the PVs The solar-rechargeable electric energy storage systems (SEESSs), which can simultaneously harvest and store solar energy, are considered a promising next-generation renewable energy supply system. However, the difficulty in meeting the demands of higher overall photoelectric conversion and storage efficiency (PCSE) with both high power density and large energy density in the current SEESSs severely limit their practical application. Herein, a new class is demonstrated of portable and highly efficient SEESS that uniquely integrates a perovskite solar module (PSM) and an aluminum-ion batter...