Feedback-driven online homework systems provide students with a comprehensive set of practice questions that can accompany and enhance other instructional resources. However, the available e-homework systems do not contain content that aligns well with our course objectives, provide too few questions in key areas, and use assessment format(s) that do not match the ones used on our exams. Motivated to create our own questions, we used this gap as an opportunity to engage students in constructing and reviewing course-aligned content within a commercial e-homework platform. The students successfully generated approximately 1,000 largely open-ended organic chemistry questions, some with mechanistic and structural drawing capabilities, by modifying old exam questions. The students' questions spanned a variety of cognitive levels that skewed, as intended, toward skill-building. According to our assessment scheme, 75% of the questions were evaluated to be of the highest quality. As a consequence, we advocate that collaborating with undergraduate students in a "teaching team" can be a broadly useful way for instructors to generate high-quality instructional materials aligned with their course content.