Hybrid organic/inorganic semiconductors (HOIS) offer tremendous opportunities to control fundamental properties that underpin energy technologies. While currently there are enormous worldwide efforts exploring, exploiting and improving a narrow class of HOIS (lead-halide perovskites, such as methylammonium lead iodide), primarily for photovoltaic (PV) applications, there are opportunities to transcend this initial focus on PV research and seek deeper understanding and control of their fundamental properties. Inherent in these unique hybrid systems is the dichotomy between organic/molecular moieties (quantum chemistry) and inorganic/extended systems (solid state physics). As a result, they exhibit properties that are not solely a juxtaposition of the inorganic and organic sub-units, but are instead truly emergent phenomena, with the concomitant ability to control and design new properties by judicious choice of inorganic and organic components. This presentation will touch on efforts to control and manipulate carriers and spin in these HOIS systems. Specifically work controlling carriers and materials chemistry via the creation of 2D-3D interfaces. Work related to efforts in the Center for Hybrid Organic Inorganic Semiconductors for Energy center to manipulate spin in these systems will also be discussed with focus on efforts to examine chiral induced spin selectivity (CISS) in these materials. Recent basic material observations in chiral hybrid systems will be discussed along with demonstrations of harnessing CISS as a functional material property as an avenue to a new class of spintronic systems. Opportunities presented by controlling charge and spin with an eye towards future directions in HOIS systems will also be touched upon.