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In this work, a series of highly sensitive surface-enhanced Raman scattering substrates have been achieved based on the controllable aggregation of silver nanoparticles. In such system, hexadecylamine-capped silver nanoparticles were ink-jet printed on glass substrates and subsequently dipped into methanol solution. An aggregation was induced due to preferential dissolution of hexadecylamine into methanol and partial removal of the protective layers on silver nanoparticle surfaces, which exhibited stable and controllable Raman enhancement effect. This strategy could be further extended to construct various chemical and biological functional sensors.