A high percentage of electron density (denoted %-ρL), often found to be >99% for common organic molecules, correspond with an accurate natural Lewis structure.
The concept of natural orbitals was first introduced by Per-Olov Löwdin in 1955, to describe the unique set of orthonormal 1-electron functions that are intrinsic to the N-electron wavefunction.
Each valence bonding NBO σ must be paired with a corresponding valence antibonding NBO σ* (the acceptor) to complete the span of the valence space: The bonding NBOs are of the "Lewis orbital"-type (occupation numbers near 2); antibonding NBOs are of the "non-Lewis orbital"-type (occupation numbers near 0).
Weak occupancies of the valence antibonds signal irreducible departures from an idealized localized Lewis structure, which means true "delocalization effects".
[1] With a computer program that can calculate NBOs, optimal Lewis structures can be found.