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Ultrafast all-optical cross-phase modulation (XPM) associated with intersubband transition was generated by silicon ion implantation in undoped InGaAs-AlAsSb coupled double quantum wells. This transverse-magnetic-pump-induced XPM for transverse-electric probe has spectral and temporal features superior to other polarization combinations. The XPM power efficiency in the 500- μm-long implanted waveguide was evaluated to be ~ 0.054 rad/pJ . This technique based on ion implantation can be used to monolithically integrate the novel XPM with other quantum-well-based functional modules.