The thin physical profile of perovskite-based solar cells (PSCs) fabricated on flexible substrates provides the prospect of a disruptive increase in specific power (power-to-mass ratio), an important figure-of-merit for solar cells to be used in space applications. In contrast to recent reports on space applications of PSCs which focus on rigid glass-based devices, in this work we investigate the suitability of flexible PSCs for low-earth orbit (LEO) applications, where the perovskite layer in the PSCs was prepared using either a Ruddlesden−Popper precursor composition (BA 2 MA 3 Pb 4 I 13 ; BA = butylammonium, MA = m e t h y l a m m o n i u m ) o r a m i x e d -c a t i o n p r e c u r s o r c o m p o s i t i o n (Cs 0.05 FA 0.81 MA 0.14 Pb 2.55 Br 0.45 ; FA = formamidinium). The flexible PSC devices display a tolerance to high-energy proton (14 MeV) and electron (>1 MeV) radiation comparable with, or superior to, equivalent glass-based PSC devices. The photovoltaic performance of the PSCs is found to be significantly less dependent on angle-of-incidence than GaAs-based triple-junction solar cells commonly used for space applications. Results from a preliminary test of the robustness of the perovskite film when subjected to LEO-like thermal environments are also reported. In addition, a unique deployment concept integrating printed flexible solar cells with titanium−nickel based shape memory alloy ribbons is presented for thermally actuated deployment of flexible solar cells from a rolled state.