Nanoscale materials have been investigated extensively for applications in memory and data storage. Recent advances include memories based on metal nanoparticles(1), nanoscale phase-change materials(2) and molecular switches(3). Traditionally, magnetic storage materials make use of magnetic fields to address individual storage elements. However, new materials with magnetic properties addressable via alternative means (for example, electrical or optical) may lead to improved flexibility and storage density and are therefore very desirable. Here, we demonstrate that copper-doped chalcogenide nanocrystals exhibit not only the classic signatures of diluted magnetic semiconductors(4)-namely, a strong spin-exchange interaction between paramagnetic Cu2+ dopants and the conduction/valence bands of the host semiconductor-but also show a pronounced and long-lived photoinduced enhancement of their paramagnetic response. Magnetic circular dichroism studies reveal that paramagnetism in these nanocrystals can be controlled and increased by up to 100% when illuminated with above-gap (blue/ultraviolet) light. These materials retain a memory of the photomagnetization for hour-long timescales in the dark, with effects persisting up to similar to 80 K.