By engaging a compact asymmetric single slit coated with a photorefractive polymer, surface-plasmon-polariton (SPP) generation was efficiently controlled by a pump beam. In the structure, the nonlinear light–matter interaction is enhanced because of the cavity effect, which increases the sensitivity of SPPs to the surrounding dielectric. By variation of the real part of the refractive index together with an interferometric configuration, high on/off switching ratios are achieved. Moreover, the SPP generation and modulation processes are integrated in the same asymmetric single slit, which makes the device ultracompact. Experimentally, a high on/off switching ratio of >20 dB and phase variation of >π were observed with the device lateral dimension of only about 2 μm.