Bamboo crown width (CW) is a reliable index for evaluating growth, yield, health and vitality of bamboo, and light capture ability and carbon fixation efficiency of bamboo forests. Based on statistical results produced from fitting the eight basic growth functions using data from 1374 Phyllostachys pubescens in Yixing, Jiangsu Province, China, this study identified the most suitable function (logistic function) to construct a two-level mixed effects (NLME) CW model with the forest block and sample plot-level effects included as random effects in the model. Four methods for selecting sample bamboos per sample plot (largest bamboo, medium-sized bamboo, smallest bamboo, and randomly selected bamboos) and eight sample sizes (1–8 selected bamboos per sample plot) were evaluated to calibrate our NLME CW model. Using diameter at breast height (DBH), height to crown base (HCB), arithmetic mean diameter at breast height (MDBH), and height (H) as predictor variables, the model produced the best fit statistics (Max R2, min RMSE, and TRE). This model was further improved by introducing random effects at two levels. The results showed a positive correlation of CW with HCB and DBH and a negative correlation with H. The smallest two bamboo poles per sample plot used to estimate the random effects of the NLME model provided a satisfactory compromise regarding measurement cost, model efficiency, and prediction accuracy. The presented NLME CW model may guide effective management and carbon estimation of bamboo forests.