The inhibitors for acetylcholinesterase (AChE), an enzyme hydrolyzing acetylcholine in cholinergic synapses, have been used for the treatment of Alzheimer's disease (AD). Alkaloids inhibiting AChE activity are commonly found in traditional Chinese medicine (TCM), e.g. gelantamine from Lycoris radiata, berberine from Coptis chinensis, huperzine A from Huperzia serrata. Many of these alkaloids also show regulatory role on inflammation, including the suppression on neuro-inflammation. Here, we aimed to reveal the possible relationship of these alkaloids in having both anti-inflammation and anti-AChE properties, in particular the role of which in “cholinergic anti-inflammatory pathway (CAP)”. A compound database containing 1,500 alkaloids from 113 kinds of TCM was developed. By molecular docking, the database was probed for AChE-inhibitory effect. Over 200 alkaloids showing AChE binding effect were further tested by its activities in inhibition of AChE, as well as in LPS-induced inflammatory responses. Thus, the current results could provide a good foundation for further research and development of TCM alkaloids on AD treatment.