Abstract Reconfigurable memristors featuring neural and synaptic functions hold great potential for neuromorphic circuits by simplifying system architecture, cutting power consumption, and boosting computational efficiency. Building upon these attributes, their additive manufacturing on sustainable substrates further offers unique advantages for future electronics, including low environmental impact. Here, exploiting the structure–property relationship of inkjet‐printed MoS 2 nanoflake‐based resistive layer, we present paper‐based reconfigurable memristors. We demonstrate a sustainable process covering material exfoliation, device fabrication, and device recycling. With >90% yield from a 16 × 65 device array, our memristors demonstrate robust resistive switching, with >10 5 ON–OFF ratio and <0.5 V operation in non‐volatile state. Through modulation of compliance current, the devices transition into a volatile state, with only 50 pW switching power consumption. These performances rival state‐of‐the‐art metal oxide‐based counterparts. We show device recyclability and stable, reconfigurable operation following disassembly, material collection and re‐fabrication. We further demonstrate synaptic plasticity and neuronal leaky integrate‐and‐fire functionality, with disposable applications in smart packaging and simulated medical image diagnostics. Our work shows a sustainable pathway toward printable, reconfigurable neuromorphic devices, with minimal environmental footprints. image