A new type of graphene-based catalyst with rewriteable function was designed and synthesized based on poly(1vinyl-3-ethylimidazolium bromide) modified and reduced graphene oxide (denoted as poly[ViEtIm] Br-rGO). The modified polymeric ionic liquid poly[ViEtIm] Br not only acted as interlink between the polar catalytic anion and the non-polar graphene substrate, but also endowed the favorable dispersibility of poly[ViEtIm] Br-rGO in ionic liquid, leading to the adequate exposure of immobilized catalytic sites during the process of desulfurization. Moreover, due to the reversible anion-exchange property of the modified poly[ViEtIm] Br, various anions of Bronsted acids or heteropolyacids could be sequentially 'written in' or 'erased' on the nanosheets of rGO for desulfurization, thus establishing a green model for screening suitable catalysts based only on the limits of the same carrier. Such a rewriteable cycle was confirmed and monitored by characterization of TEM, FTIR spectroscopy and X-ray photoelectron spectroscopy (XPS). Based on this catalyst screening process of a rewriteable cycle, poly[ViEtIm][PW12O40]-rGO, a heteropolyanoin modified rGO, was selected as the optimized catalyst. Benefiting from the synergistic effects between rGO and acidic anions, together with the large surface area and open two-dimensional structure of rGO, poly[ViEtIm][PW12O40]-rGO was found to exhibit an excellent catalytic performance toward various sulfur-containing compounds. Furthermore, the outstanding reusability of poly [ViEtIm][PW12O40]-rGO was also displayed owing to its structural stability. It was found that the sulfur removal efficiency of DBT could still reach 98.0% after the catalyst poly[ViEtIm][PW12O40]-rGO had even been recycled eight times.