Organic room-temperature phosphorescence (ORTP), when combined with external stimuli-responsive capability, is very attractive for sensors and bio-imaging devices, but remains challenging. Herein, by doping two β-iminoenamine-BF derivatives (S-2CN and S-2I) into a 4-iodoaniline (I-Ph-NH ) crystalline matrix, the formation of S-2CN⋅⋅⋅I-Ph-NH and S-2I⋅⋅⋅I-Ph-NH halogen bonds leads to bright-red RTP emissions from these two host-guest doped crystals (hgDCs) with quantum efficiencies up to 13.43 % and 15.96 %, respectively. Upon treatment with HCl, the competition of I-Ph-NH ⋅HCl formation against S-2I⋅⋅⋅I-Ph-NH halogen bonding switches off the red RTP from S-2I/I-Ph-NH hgDCs, whereas the stable halogen-bonded S-2CN⋅⋅⋅I-Ph-NH ensures red RTP from S-2CN/I-Ph-NH hgDCs remains unchanged. A security protection luminescence pattern by using these different HCl-responsive RTP behaviors was designed.