Intercropping plays an essential role in enhancing the biodiversity and stability of agroecosystems. The aim of this study was to investigate the optimal pattern and arrangement in safflower/chickpea intercropping in a semi-arid region of Iran. Treatments evaluated in this study were sole cropping of safflower and chickpea, their replacement series (4:4, 2:2, 1:1, 3:1, 1:3), and additive series (20% and 40% of chickpea in both situations in the middle (I) and around (II) of safflower rows). The results showed that the greatest intercropping indices such as land equivalent ratio (LER), area time equivalent ratio (ATER), and system productivity index (SPI) belonged to 40%I additive intercropping pattern. These mentioned values were 1.9, 1.8, and 307.8, respectively. The intercropping patterns had a significant effect on the fatty acid composition of safflower oil. Unsaturated fatty acids including linoleic and oleic acids were higher in the intercropping patterns, whereas, saturated fatty acids consisting of palmitic, myristic, and stearic acids were higher in the safflower sole cropping. Linoleic and oleic acid increased by 9.6% and 16.1% in 40%I compared to sole cropping. Overall, 40%I additive intercropping pattern is more promising in grain and oil yield, intercropping indices, and oil quality than the other intercropping patterns.