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This study uses the inclusion complex method to import nonlinear optical (NLO) chromophores, disperse red1 (DR1), and spiropyran (SP), into the γ-CD cavity of the γ-cyclodextrin polymer (γ-CDP) to prepare orderly aligned nonphotocontrollable and photocontrollable nonlinear optical polymers. Calculations support the ultraviolet/visible analyses and suggest the formation of the 1 : 2 DR1/γ-CDP and 1 : 2 SP/γ-CDP inclusion complexes. Upon complexation, the DR1 and SP molecules are free to align themselves along an applied electric field and show high order parameters of approximately 0.48 and 0.20, respectively. Reversible photochromic reactions exhibit that the SP/γ-CDP complex still retains the photochromic properties following corona poling.