We present an interpretation of Fermi‐orbital descriptors (FODs) and argue that these descriptors carry chemical bonding information. We show that a bond order derived from these FODs agrees well with reference values, and highlight that optimized FOD positions used within the Fermi‐Löwdin orbital self‐interaction correction (FLO‐SIC) method correspond to expectations from Linnett's double‐quartet theory, which is an extension of Lewis theory. This observation is independent of the underlying exchange‐correlation functional, which is shown using the local spin density approximation, the Perdew–Burke–Ernzerhof generalized gradient approximation (GGA), and the strongly constrained and appropriately normed meta‐GGA. To make FOD positions generally accessible, we propose and discuss four independent methods for the generation of Fermi‐orbital descriptors, their implementation as well as their advantages and drawbacks. In particular, we introduce a re‐implementation of the electron force field, an approach based on the centers of mass of orbital densities, a Monte Carlo‐based algorithm, and a method based on Lewis‐like bonding information. All results are summarized with respect to future developments of FLO‐SIC and related methods. © 2019 The Authors. Journal of Computational Chemistry published by Wiley Periodicals, Inc.