What happens to spin-polarized electrons when they enter a superconductor? Superconductors at equilibrium and at finite temperature contain both paired particles (of opposite spin) in the condensate phase as well as unpaired, spin-randomized quasiparticles. Injecting spin-polarized electrons into a superconductor (and removing pairs) thus creates both spin and charge imbalances 1-7 , which must relax when the injection stops, but not necessarily over the same time (or length) scale. These different relaxation times can be probed by creating a dynamic equilibrium between continuous injection and relaxation; this leads to constant-in-time spin and charge imbalances, which scale with their respective relaxation times and with the injection current. Whereas charge imbalances in superconductors have been studied in great detail both theoretically 8 and experimentally 9 , spin imbalances have not received much experimental attention 6,10,11 despite intriguing theoretical predictions of spin-charge separation effects 12,13 . Here we present evidence for an almost-chargeless spin imbalance in a mesoscopic superconductor.A pure spin imbalance in a superconductor can be understood in the following manner: imagine injecting spin-randomized electrons continuously into a small superconducting volume and taking out Cooper pairs. The number of electron-like quasiparticles increases, that is, their chemical potential µ QP rises whereas that of the Cooper pairs µ P drops by the same amount to conserve particle number. This charge imbalance was first observed in a pioneering experiment, where µ QP − µ P was measured 1,2,14 . (Hereafter µ P ≡ 0, that is, all chemical potentials are measured with respect to that of the condensate.) If the injected electrons are (or become) spin-polarized, in general µ QP↑ = µ QP↓ = µ P , we can define a charge imbalance µ C ≡ (µ QP↑ + µ QP↓ )/2 and spin imbalance µ S ≡ (µ QP↑ − µ QP↓ )/2 (ref. 13). If charge relaxes faster than spin, a situation may arise in which µ C = 0 while µ S = 0. This is our chargeless spin imbalance. (See Supplementary Information for more details.) In the experiment, µ QP↑ − µ P and µ QP↓ − µ P are measured as a voltage drop between a spin-sensitive electrode and the superconductor.We implement a mesoscopic version of an experiment proposed in refs 12,13; this offers two practical advantages: the detector can be placed within a spin relaxation length λ S of the injection point and all out-of-equilibrium signals are enhanced by the small injection volume. In diffusive transport, λ S = (Dτ S2 ) 1/2 , where τ S2 is the spin relaxation time and D the diffusion constant (∼5 × 10 −3 m 2 s −1 in our samples 15 ). Our samples are FISIF lateral spin valves 16 , where the F are ferromagnets (Co), the I are insulators (Al 2 O 3 ) and S is the superconductor (Al), as shown in Fig. 1a. The SIF junctions have sheet resistances of ∼1.6 × 10 −6 cm 2 (corresponding to a barrier transparency T ∼ 5 × 10 −5 ) and tunnelling is the main transport mechanism through the insulator. By sweeping an...