Linqing brick is quite popular in Chinese history. In 2008, “The manufacturing process of Linqing brick” was selected as the intangible cultural heritage list in China. Currently, identifying the origin of Linqing brick represents an important issue to be investigated in the field of archeology and architectural history research in China, as it could be used to verify certain assumptions regarding the history of heritage buildings, the resolution for which cannot be obtained by examining the historical documents. Hand Held X-ray fluorescence (HH-XRF) spectrometry enables the in-situ determination of the main elements and concentrations of Linqing brick in a rapid non-destructive manner. HH-XRF may prove to be significant in identifying the origin of Linqing brick. However, HH-XRF could be influenced by certain factors and may be capable of measuring only the element concentrations of the surface for the brick in situ. Which method would provide the most reliable data is an important concern. The aim of the present study was to verify the reliability of HH-XRF and to systematically evaluate the different factors influencing measurement precision and accuracy, in order to assist with scientific advice for the usage of HH-XRF. Four experiments were performed to determine the influencing factors and to assess reliability through cross-validation using inductively coupled plasma optical emission spectrometry (ICP-OES). Finally, the reliability of HH-XRF was ensured, and the scientific advice regarding its application in determining the concentrations of the main elements of Linqing brick was provided.