A variety of bionic vacuum suckers with papillae structures of different parameters were developed to improve the attachment performance of vacuum suckers. The oral sucker of the suckermouth catfish served as the bionic prototype and bionic suckers were made by taking the diameter of papillae, the number of single rows of papillae, the center distance between adjacent rows of papillae, and the distance between the outermost row of papillae and the edge as influencing factors. The single-factor tests and response surface tests were carried out respectively with the growth rates of vertical and horizontal attachment forces as the response values. Twenty-five groups of bionic suckers and one group of standard suckers were fabricated and tested for attachment forces. The experimental results revealed that the bionic suckers had higher vertical and horizontal attachment forces than standard suckers and that their maximum growth rates for these forces were 5.16% and 59.87%, respectively. This suggested that the bionic suckers had better attachment performance. The significant orders of the factors affecting response values were established and their interaction was also analyzed. Besides, the optimal parameter combination of papillae structures of the bionic suckers with optimal vertical and horizontal attachment properties was obtained, respectively. Finally, the influence mechanism of papillae structures on the attachment properties of bionic suckers was analyzed. The studies can serve as a guide for the application of bionic suckers in agricultural production areas such as fruit picking and handling, and the improvement of attachment performance of associated machinery.