Nanoscale multifunctional perpendicular organic spin valves have been fabricated. The devices based on an La 0.7 Sr 0.3 MnO 3 /Alq3/Co trilayer show resistive switching of up to 4-5 orders of magnitude and magnetoresistance as high as -70% the latter even changing sign when voltage pulses are applied. This combination of phenomena is typically observed in multiferroic tunnel junctions where it is attributed to magnetoelectric coupling between a ferromagnet and a ferroelectric material. Modeling indicates that here the switching originates from a modification of the La 0.7 Sr 0.3 MnO 3 surface. This modification influences the tunneling of charge carriers and thus both the electrical resistance and the tunneling magnetoresistance which occurs at pinholes in the organic layer.In the past years a number of multiferroic tunnel junctions have been demonstrated in which tunneling magnetoresistance (TMR) and total device resistance can be modulated by a voltage pulse. 1,2 The effects are typically explained by tunneling electroresistance (TER) due to a ferroelectric barrier which changes the total resistance and magnetoelectric coupling at the interface between ferroelectric barrier and ferromagnetic contact which changes the TMR in magnitude and sometimes in sign. We observe the same functionality in organic spin valves (OSVs, Fig. 1), which after applying a voltage pulse may change the device resistance by three orders of magnitude or more and modulate their magnetoresistance (MR) from +26% to -38% which is a much larger effect than observed in Refs. 1 or 2. Nevertheless, the absence of a ferroelectric layer in our devices excludes both TER and magnetoelectric coupling as possible explanation. It should, however, be noted that our devices and those from Refs. 1 and 2 have a La 0.7 Sr 0.3 MnO 3 (LSMO) bottom electrode as a common property.FIG. 1: MR traces of a nanosized OSV (LSMO/Alq3/MgO/Co/Ru with 20/12/3/30/10 nm in thickness) for two different resistance states after different voltage pulses taken at 4.3 K. The resistance changes by approx. three decades and the relative MR exhibit a sign reversal from +26% to -38%. Already in 2011 the simultaneous observation of magnetoresistance and resistive switching (RS) has been reported for organic spin valves by Prezioso et al. 3,4 In this case the devices were LSMO/Alq3/Co-based spin valves showing a relative MR of -20% in the initial state. By applying 2 voltage pulses the overall device resistance was increased while the relative MR decreased without changing shape or sign. The device resistance could be increased by two decades while the MR was completely suppressed. A possible explanation suggested by Prezioso et al. was the blocking of filaments or charge trapping in combination with giant magnetoresistance (GMR) and spin injection as a prevalent transport mechanism, however, no clear identification of the underlying physics was possible. Recent results from our own group in structures with only one ferromagnetic electrode (LSMO) also demonstrated RS. However, in thi...