•Notable correlations between pellicle colors and phenolics in kernel without pellicle.•Positive correlations between TPCs of three forms in pellicle and their colors.•Dark walnuts with high contents of flavanols, flavones and flavonols in free form. Although walnut kernels are a rich source of phenolic compounds, little is known about the profiles of phenolic compound forms in various colored-pellicle walnuts, which may be important for product development and utilization. In this work, the free, esterified and bound forms of phenolic compounds in various colored-pellicle walnuts were identified using ultra-high-performance liquid chromatography coupled to tandem mass spectrometry ((UHPLC-MS/MS). The total phenolics (TPCs) in pellicle, kernel without pellicle and whole kernel (with pellicle) were presented in the free form (62.6%) and bound form (1.30 %–12.2 %). Positive correlations were found between the TPCs of three forms in pellicle and the pellicle color, with correlation coefficients of 0.920, 0.990 and 0.940. In addition, the phenolic compounds in free form in the whole kernel (with dark pellicle) demonstrated notable advantages in flavanols, flavones and flavonols contents, particularly (+)-catechin (C) (40.7 μg/g) and epicatechin (EC) (25.8g/g), which were 2–153 times higher than other phenolic compounds in free form. Furthermore, the dark group of esterified phenolic acids showed advantages, particularly ellagic acid (428 μg/g) and gallic acid (130 μg/g).