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We report the manufacturing of an (ultra-)thin foil target made of conjugated polymer, poly(9,9′-dioctylfluorene-co-benzothiadiazole) (F8BT), and the simultaneous observation of laser-accelerated ions and second harmonic radiation, when irradiated with ultrahigh-contrast laser pulse at a maximum intensity of 4 × 1019 W/cm2. Maximum proton energy of 8 MeV is achieved along the target normal direction. Strong second harmonic with over 6% energy ratio compared to fundamental is emitted along the specular direction. Two-dimensional particle-in-cell simulations confirm the simultaneous generation of protons and high-order harmonics, which demonstrates the feasibility of applications requiring particle and radiation sources at once, effectively using the same laser and target.