Beijing-Tianjin-Hebei　and　the　surrounding　area　(BTHSA)　shows　the　poorest　air　quality　in　China,　reflected　in　substandard　PM2.5　and　increasingly　pronounced　O3　pollution,　stressing　the　urgency　for　regional　cooperation　and　collaborative　control　of　PM2.5　and　O-3.　With　the　aim　to　explore　the　cooperative　regions　and　response　mechanisms　of　PM2.5　and　O-3　in　BTHSA,　this　study　applied　multiple　mathematical　models　and　analytical　indicators　to　multiple　data　sources,　including　applying　self-organizing　map　(SOM),　response　surface　model　(RSM),　random　forest　(RF),　distributed　lag　nonlinear　models　(DLNMs),　and　meta-analysis,　on　ground　observations　of　air　quality　and　meteorology,　ozone　monitoring　instrument　(OMI)　observations,　and　air　pollutant　emission　inventory.　The　results　revealed　that　BTHSA　exhibited　clear　regional　characteristics　of　air　pollution　and　can　be　divided　into　four　clusters　for　enhanced　intercity　cooperation.　Over　2015-2020,　anthropogenic　factors　played　more　important　roles　than　meteorological　ones　on　the　alleviation　of　PM2.5　and　the　deterioration　of　O-3.　RSM　based　on　observations　and　RF　based　on　emissions　both　suggested　that,　in　the　near　future,　strengthened　abatement　of　SO2,　PM2.5　and　VOC　can　be　beneficial　for　controlling　PM2.5　and　O-3　pollution,　while　intensive　NOx　reduction　in　PM2.5-dominant　months　and　mitigatory　NOx　reduction　in　O3-dominant　months　should　be　formulated　before　certifying　an　obvious　transition　of　O-3-NOx-VOC　sensitivity.　This　study,　with　multi-model　and　multi-data　fusion,　can　be　expected　to　provide　synthesized　fact-and　science-based　guidance　for　the　next-stage　collaborative　control　of　PM2.5　and　O-3　in　BTHSA.