Plastic waste has been becoming a severe environmental issue. Developing low-cost and facile strategy to converse them into the high value-added materials for remediation of ecosystem is a big challenge. In this manuscript, Polystyrene foam waste (PSF) was employed as starting material to react with the different mass ratio of cyanuric chloride (CC) to synthesize a series of hyper-cross-linked polymers (HPPCs). HPPCs were porous polymers and mainly composed of micro-pores and meso-pores. Their apparent surface areas (SBET) and pore volumes were in range of 622.9 ± 11 and 719.2 ± 15 m2 g−1, 0.87 and 1.01 cm3 g−1, respectively. The SBET and pore volume could be tuned by the mass ratio of PSF and CC. Adsorption experiments revealed that HPPC-3 showed high adsorption quantities of rhodamine B (RhB) and malachite green (MG) with the maximum adsorption capacities of 2354.0 ± 60.8 and 1331.9 ± 30.6 mg g−1, respectively. The adsorption isotherm and kinetics data suggested that the adsorption behaviors of RhB and MG on HPPC-3 followed the Langmuir models and pseudo-second-order models. Additionally, HPPC-3 displayed high adsorption capacity of iodine vapor up to 188 ± 3.2 wt%. Therefore, this work suggested a new approach for converting plastic waste into the promising adsorbent for removal of dyes and radioactive iodine vapor from contaminated ecosystem.