In tissue engineering, cell-adhesion peptides (CAPs) such as the ubiquitous arginine-glycine-aspartic acid (RGD) sequence have allowed the functionalization of synthetic materials to mimic macromolecules of the extracellular matrix (ECM). However, the variety of ECM macromolecules makes it challenging to reproduce all of the native tissue functions with only a limited variety of CAPs. Screening of libraries of CAPs, analogous to high-throughput drug discovery assays, can help to identify new sequences directing cell organisation. However, challenges to this approach include automation of cell seeding in three dimensions and characterization methods. Here, we report a method for robotically generating a library of 16 CAPs to identify microenvironments capable of directing a chain-like morphology in olfactory ensheathing cells (OECs). OECs are of particular interest for spinal cord injury to guide axon growth. This approach resulted in the identification of two CAPs not previously reported to interact with OECs to direct their morphology into structures suitable for axon guidance. The same screening approach should be applicable to any range of cell types to discover new CAPs to direct cell fate or function.© 2020 IOP Publishing Ltd.