Microwave (MW) pretreatment as an energy-efficient method to enhance the production of nanofibrillated cellulose (NFC) from lime (Citrus aurantifolia Swingle) residue after juice extraction is proposed. NFC was prepared by subjecting lime residue to MW pretreatment for up to 3 rounds; this was followed by high-shear and high-pressure homogenization. Repeated application of MW pretreatment helped remove non-cellulosic components and resulted in an increased cellulose content and crystallinity index but a decrease in fiber diameter. Freshly prepared NFC sample exhibited gel-like behavior. G′ and G″ of suspension prepared from dried NFC markedly decreased, indicating the loss of gel-like property upon drying. Proper pectin molecular weight as well as pectin content were noted to play an important role in controlling aggregation of NFC during drying and hence water redispersibility of dried NFC. Significant amounts of pectin and limonin could be recovered and utilized as co-products after the first round of MW pretreatment.