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This paper reports the finding of an investigation of a surface molecular self-assembly strategy for molecular imprinting of polymer nanowires/nanotubes. It has been demonstrated that 2,4,6-trinitrotoluene (TNT) templates were spontaneously assembled onto aminopropyl group-modified alumina pore walls by a strong charge-transfer complexing interaction between amino groups and electron-deficient nitroaromatics, forming a novel basis of surface molecular imprinting. While an additional amount of TNT templates was further replenished into a precursor mixture, a stepwise progressive polymerization was designed toward the controllable preparation of TNT-imprinted polymer nanowire/nanotube arrays in an alumina membrane. The imprinted nanowires/nanotubes with a high density of surface-imprinted sites and regular interior sites exhibit the high capacity of binding TNT molecules, which is nearly 2.5-3.0-fold that of normal imprinted particles. Moreover, the imprinted nanotubes and nanowires have ~6- and 4-fold increase in the rate of binding TNT molecules, respectively. The combination of surface molecular assembly with nanostructures in the imprinting technique can create more effective recognition sites than the only use of porogens in traditional approaches. This novel, facile strategy reported herein can be further expected to fabricate various molecular recognition nanoarrays for sensing or analytic applications. [ABSTRACT FROM AUTHOR]