Herein,　an　attempt　was　made　to　modulate　the　properties　of　NiO　oxides　towards　methane　combustion.　For　this　purpose,　appropriate　content　of　copper　was　introduced　into　the　NiO　lattice　to　generate　Cu–Ni　solid　solution,　in　view　of　the　similarities　in　atomic-size　and　electronegativity　between　copper　and　nickel.　This　delivered　more　unsaturated　nickel　atoms　and　reduced　the　nanoparticle　size　of　NiO,　generating　more　lattice　defects.　Also,　the　oxygen　binding　energy　was　significantly　lowered　stemming　from　the　creation　of　Ni–O–Cu　linkage,　and　the　interaction　between　CuO　and　NiO.　Consequently,　larger　amount　of　active　surface　adsorbed　oxygen　sites　were　given　and　the　reducibility　of　NiO　was　considerably　enhanced　for　bimetallic　systems　compared　with　pure　NiO.　Meanwhile,　the　surface　acid-base　properties　were　adjusted　over　samples　after　the　addition　of　copper,　attributed　to　the　charge　redistribution　among　the　oxygen　and　metal　atoms.　These　effects　accounted　for　the　preferred　activity,　water-resistance,　and　durability　for　Cu-promoted　NiO　catalysts.　©　2021　Hydrogen　Energy　Publications　LLC