Anisotropic multicomponent polymers (AMPs) with improved and synergetic functions are a unique class of the most intriguing materials with versatile applications. Thus, the synthetic strategy for establishing AMPs with tunable functions and compositional complexities is highly desirable. Herein, we report a new paradigm for the facile and controllable in situ synthesis of dual-component poly(TMPTA-co-HEA) and poly(HEA-co-NVP) polymers (TMPTA = trimethylolpropane triacrylate, HEA = 2-hydroxyethyl acrylate, NVP = 1-vinyl-2-pyrrolidone) by utilizing laser-ignited anisotropic biphase frontal polymerization (FP). Once anisotropic biphase FP was initiated, no further energy was required for the polymerization, providing a simple, rapid and cost-effective approach for the synthesis of AMPs. The dependence of the frontal velocities and temperatures on initiator concentrations and the monomers weight ratios have been discussed in detail. More interestingly, an operable fluorescent two-dimensional (2D) code was constructed through the introduction of fluorescent dye and quantum dots into the bilayer film. And, the as-prepared 2D code demonstrated the capability in chemical recognition toward organic amines. It could be believed the methodology developed in this work may open a hopeful avenue to design other kinds of AMPs with various desirable applications.