Deep-UV　nonlinear　optical　(NLO)　materials　have　attracted　much　academic　and　technical　attention　due　to　their　capability　of　producing　coherent　light　of　wavelengths　below　200　nm.　As　a　well-known　branch　of　NLO　materials,　researchers　have　obtained　many　deep-UV　NLO　crystals　with　superior　properties　in　π-conjugated　system　materials　(such　as　borate　systems　and　carbonate　systems).　However,　due　to　structural　and　property　limitations,　the　research　developments　have　encountered　difficulties　in　balancing　NLO　properties.　Recently,　scientists　started　to　pay　attention　to　the　non-π-conjugated　system　of　deep-UV　NLO　materials.　As　far　as　we　know,　the　non-π-conjugated　deep-UV　NLO　materials　could　be　divided　into　six　categories:　phosphates,　sulfates,　borophosphates,　borosilicates,　fluorides,　and　silicates.　This　review　focuses　on　the　research　advances　of　deep-UV　NLO　materials　with　non-π-conjugated　functional　groups　and　summarizes　and　discusses　the　deep-UV　NLO　crystals　on　the　basis　of　the　performance　criteria　of　＇deep-UV　transmission-large　NLO　effect-large　birefringence＇.　By　analyzing　the　structure-property　relationships　of　these　materials,　we　summarize　the　microscopic　mechanism　restricting　the　balance　of　properties　and　new　functional　groups,　which　may　provide　new　ideas　and　help　the　explorations　of　deep-UV　NLO　materials.　©　2021　American　Chemical　Society.