Developing of new polymeric materials for the sensitive and rapid detection of trace protein biomarkers has attracted increasing attention in biomedical fields. Herein, series of in situ photoinduced polymer graftings were developed for sensitive detection of protein biomarkers by using featured cascade amplification of liquid crystal (LC) signals. The limit-of-detection (LOD) for native bovine serum albumin (BSA) molecules is around 10 μg/mL in a LC biosensor before signal amplification. Upon the cascade amplification using surface-grafted polymers, poly[poly(ethylene glycol) methacrylate] grafting ( s-P(PEGMA)) exhibits superior amplification ability (104-fold lower than native BSA) than the other two graftings of poly(2-hydroxyethyl methacrylate) ( s-PHEMA) and poly(methacrylic acid) ( s-PMAA; 102-fold lower than native BSA). The contact angles of water and LC on the s-P(PEGMA) grafting show significant difference in comparison with s-PHEMA and s-PMAA graftings ( p < 0.05), implying interfacial energies of the grafted polymers may dictate the orientational transition of LCs. The clinical urine samples collected from the patients with proteinuria were also used to confirm the feasibility of the polymer-amplified LC sensors for practical protein assays. The present work reveals that in situ photoinduced polymer grafting is one promising method to amplify the signals of LC biosensors for the rapid and sensitive detection of trace protein biomarkers.