In　this　paper,　a　novel　core@shell　nanosphere　(TiO2@CoAl-LDH)　based　on　layered　double　hydroxide　(LDH)　combined　with　a　nano-TiO2　semiconductor　was　synthesized　and　introduced　to　cementitious　materials　via　spraying　technology　and　a　smearing　method.　The　compatibility　with　a　cementitious　matrix　and　the　effects　of　TiO2@CoAl-LDH　on　cement　hydration,　surface　microstructure,　and　the　microscopic　mechanical　properties　of　mortar　were　investigated　by　AFM,　microhardness　testing,　FESEM,　and　BET　analysis.　Meanwhile,　the　effects　of　TiO2@CoAl-LDH　introduction　methods　on　the　photocatalytic　performance　and　durability　of　the　photocatalyst　were　systematically　evaluated　by　methylene　blue　(MB)　removal　ratio　and　wear　testing.　The　results　show　that　TiO2@CoAl-LDH　exhibits　enhanced　compatibility　with　cementitious　matrices　and　a　higher　photocatalytic　capacity　than　individual　CoAl-LDH　and　nano-TiO2.　The　photocatalytic　mortar　prepared　via　spraying　technology　(CM-C)　displays　a　higher　photocatalytic　capacity　than　that　prepared　via　the　smearing　method　(CM-S).　Among　them,　the　mortar　with　two　layers　of　photocatalytic　coatings　(CM-C2)　has　the　highest　MB　removal　ratio,　which　reached　95.1%　within　120　min　of　UV-visible　light　irradiation.　While　on　the　other　hand,　the　wear　test　revealed　that　the　smeared　mortar　has　a　higher　photocatalytic　capacity　and　better　photocatalyst　durability　than　the　sprayed　mortar.　This　work　is　expected　to　contribute　to　the　development　of　multifunctional　sustainable　building　materials.