The　development　of　efficient　and　stable　non-noble　metal-based　catalysts　for　low-temperature　methane　combustion　is　extremely　important　and　still　a　profound　challenge.　Herein,　high-performance　Ni1-xZrxO2-δ　solid　solution　nanocatalysts　were　prepared　through　a　homogeneous　co-precipitation　strategy,　where　the　hydrolysis　of　CO32-　was　controlled　to　facilitate　the　dispersion　and　interaction　of　Ni　and　Zr　components.　The　structural　and　surface　properties　of　nanocatalysts　were　facilely　tuned　by　modulating　the　Zr　doping　content.　An　optimized　incorporation　of　Zr　into　the　NiO　lattice　endowed　the　Ni0.89Zr0.11O2-δ　nanocatalyst　with　a　small　crystallite　size,　large　specific　surface　area,　and　simultaneously　increased　surface　acidic-basic　sites.　Moreover,　abundant　active　Ni2+　and　surface　oxygen　species　were　generated　due　to　the　promoted　conversion　of　Ni3+　to　Ni2+,　which　played　pivotal　roles　in　the　adsorption/activation　of　methane　and　further　oxidation　of　reaction　intermediates　to　CO2.　Consequently,　Ni0.89Zr0.11O2-δ　exhibited　an　excellent　low-temperature　activity,　high　CO2　selectivity,　and　superior　catalytic　stability　under　both　dry　and　wet　conditions.　©　2021　American　Chemical　Society.　All　rights　reserved.