With the advent and widespread deployment of Multimodal Large Language Models (MLLMs), ensuring their safety has become increasingly critical. To achieve this objective, it requires us to proactively discover the vulnerability of MLLMs by exploring the attack methods. Thus, structure-based jailbreak attacks, where harmful semantic content is embedded within images, have been proposed to mislead the models. However, previous structure-based jailbreak methods mainly focus on transforming the format of malicious queries, such as converting harmful content into images through typography, which lacks sufficient jailbreak effectiveness and generalizability. To address these limitations, we first introduce the concept of "Role-play" into MLLM jailbreak attacks and propose a novel and effective method called Visual Role-play (VRP). Specifically, VRP leverages Large Language Models to generate detailed descriptions of high-risk characters and create corresponding images based on the descriptions. When paired with benign role-play instruction texts, these high-risk character images effectively mislead MLLMs into generating malicious responses by enacting characters with negative attributes. We further extend our VRP method into a universal setup to demonstrate its generalizability. Extensive experiments on popular benchmarks show that VRP outperforms the strongest baseline, Query relevant and FigStep, by an average Attack Success Rate (ASR) margin of 14.3% across all models.