The rapid advancement of multimodal large language models (MLLMs) has led to breakthroughs in various applications, yet their security remains a critical challenge. One pressing issue involves unsafe image-query pairs--jailbreak inputs specifically designed to bypass security constraints and elicit unintended responses from MLLMs. Compared to general multimodal data, such unsafe inputs are relatively sparse, which limits the diversity and richness of training samples available for developing robust defense models. Meanwhile, existing guardrail-type methods rely on external modules to enforce security constraints but fail to address intrinsic vulnerabilities within MLLMs. Traditional supervised fine-tuning (SFT), on the other hand, often over-refuses harmless inputs, compromising general performance. Given these challenges, we propose Secure Tug-of-War (SecTOW), an innovative iterative defense-attack training method to enhance the security of MLLMs. SecTOW consists of two modules: a defender and an auxiliary attacker, both trained iteratively using reinforcement learning (GRPO). During the iterative process, the attacker identifies security vulnerabilities in the defense model and expands jailbreak data. The expanded data are then used to train the defender, enabling it to address identified security vulnerabilities. We also design reward mechanisms used for GRPO to simplify the use of response labels, reducing dependence on complex generative labels and enabling the efficient use of synthetic data. Additionally, a quality monitoring mechanism is used to mitigate the defender's over-refusal of harmless inputs and ensure the diversity of the jailbreak data generated by the attacker. Experimental results on safety-specific and general benchmarks demonstrate that SecTOW significantly improves security while preserving general performance.