An efficient cropping system optimizes the use of available resources by maximizing productivity per unit area and time while minimizing environmental impacts. Therefore, identifying location-specific cropping systems that enhance productivity, profitability, and soil health is crucial for sustainable agricultural development in eastern India. Therefore, the present study evaluated the performance of diversified cropping systems under the agro-ecological conditions of Bihar, India. A 2-year field experiment (2019–2021) was conducted at the Crop Research Farm of Dr. Rajendra Prasad Central Agricultural University, Pusa, located in Samastipur, Bihar, India. The experiment was laid out in a randomized complete block design with 10 cropping systems and three replications. System performance was evaluated using indicators such as rice equivalent yield (REY), apparent water productivity (AWP), economic returns, and benefit–cost ratio. The results revealed significant variation among cropping systems in terms of productivity and economic performance. The rice–(potato + maize) (CSSc3) cropping system recorded the highest system productivity with a 231.66% increase over the rice–wheat cropping system (RWCS), followed by soybean–potato–sunflower (CSSc8) with a 187.69% increase, with both systems remaining statistically at par and significantly superior to other cropping sequences. Apparent water productivity was also the highest in CSSc3, showing a 169.0% increase over RWCS, followed by CSSc8 (140.2% increase). Economic analysis further revealed that CSSc3 achieved the highest net returns with a 232.2% increase over RWCS, followed by CSSc8 (181.7% increase). Similarly, the benefit–cost ratio was the highest in CSSc3 (60.2% increase over RWCS), while CSSc8 recorded a 43.1% increase, indicating superior economic efficiency of diversified systems. Overall, the findings indicate that diversification of rice-based cropping systems with high-value crops can significantly improve productivity, water-use efficiency, and farm profitability. The rice–potato + maize system emerged as the most efficient and economically viable cropping sequence for enhancing the sustainability of agricultural production in the eastern Indo-Gangetic Plains.