Organic-inorganic　hybrid　halides　have　attracted　widespread　attention　in　optics,　electricity,　magnetism.　In　particular,　some　of　them　can　have　a　combination　of　luminescence　and　switching　characteristics,　providing　a　potential　for　a　single　device　unit　to　meet　multiple　application　requirements.　Herein,　we　reported　two　novel　organic-inorganic　hybrid　single-crystals　(CTA)(2)ZnCl4　(1;　CTA=3-chloro-2-hydroxypropyltrimethylammonium)　and　(CTA)(2)[InCl5(H2O)]　.　H2O　(2),　exhibiting　long　lifetime　blue　emission　upon　UV　excitation.　Systematic　characterizations　of　the　compounds　including　crystal　structure,　phase　transition,　thermal,　and　photoluminescence　properties　were　carried　out.　DSC　tests　detected　that　1　had　a　reversible　phase　transition　accompanied　by　obvious　heat　anomaly,　at　411/391　K　on　the　heating/cooling　process,　leading　to　its　good　switchable　dielectric　response　with　striking　anisotropy　along　various　crystallographic　axis.　This　work　offered　a　new　example　on　the　effective　design　of　multifunctional　response　materials.