As a form of dementia, Alzheimer's disease (AD) suffers from no efficacious cure, yet AD treatment is still imperative, as it ameliorates the symptoms or prevents it from deteriorating or maintains the current status to the longest extent. The human brain is the most sensitive and complex organ in the body, which is protected by the blood–brain barrier (BBB). This yet induces the difficulty in curing AD as the drugs or nanomaterials that are much inhibited from reaching the lesion site. Thus, BBB crossing capability of drug delivery system remains a significant challenge in the development of neurological therapeutics. Fortunately, nano‐enabled delivery systems possess promising potential to achieve multifunctional diagnostics/therapeutics against various targets of AD owing to their intriguing advantages of nanocarriers, including easy multifunctionalization on surfaces, high surface‐to‐volume ratio with large payloads, and potential ability to cross the BBB, making them capable of conquering the limitations of conventional drug candidates. This review, which focuses on the BBB crossing ability of the multifunctional nanomaterials in AD diagnosis and treatment, will provide an insightful vision that is conducive to the development of AD‐related nanomaterials.