The majority of undergraduates own a smartphone, yet fewer than half view it as a valuable learning technology. Consequently, a digital laboratory notebook (DLN) was developed for an upper-division undergraduate biochemistry laboratory course using the free mobile application Evernote. The cloud-based DLN capitalized on the unique features of smartphones (i.e., photo uploading, audio capture, dictation) and could also be accessed from any Internet-connected device (i.e., tablet, laptop, desktop). This cross-platform flexibility enabled a “Bring Your Own Device” philosophy in the course, leveraging the educational power of students’ personal devices. The DLN served as a secure data management system, where any file could be attached, edited, and analyzed. The DLN also accommodated freehand drawing. A postsemester survey indicated that the cloud connectivity of the DLN facilitated greater collaboration between students and enhanced the quality of their communication with the instructor compared with traditional paper notebooks. Given the option, 70% of students reported that they would choose a DLN over a paper notebook in the future. By using a DLN, students further cultivated their digital and chemical information literacy, which is important to develop as the healthcare and industrial sectors continue to digitize their workflows.