Recent advancements in Large Multimodal Models (LMMs) have significantly improved multimodal understanding and generation. However, these models still struggle to generate tightly interleaved image-text outputs, primarily due to the limited scale, quality, and instructional richness of current training datasets. To address this, we introduce InterSyn, a dataset that features: (1) large scale, comprising 1.8M multimodal samples; (2) high quality, supported by our proposed Self-Evaluation with Iterative Refinement (SEIR) method for rigorous automated quality refinement; (3) rich instructional diversity, ensured through diverse well-designed question templates, based on human preferences and covering a 3500-topic hierarchy. These characteristics make InterSyn particularly well-suited for training LMMs in interactive image-text generation capabilities. To evaluate the capabilities, we propose SynJudge, a reliable automatic evaluator that aligns closely with human judge and outputs four interpretable scores: Text Content Completeness (TCC), Image Content Completeness (ICC), Image Quality (IQ), and Image-Text Synergy (ITS). These scores are complementary, covering both content and quality as well as cross-modal interaction, thereby forming a comprehensive evaluation framework. Experimental results on InterSyn subsets of up to 200K samples show that 25K-50K already yield substantial improvements, while scaling to 100K/200K brings further gains in TCC, ICC, and especially ITS, highlighting InterSyn's: (1) scalability, as performance consistently improves with more data; (2) efficiency, as significant gains are achievable even with smaller subsets, making it accessible to researchers with varying computational resources.