Forest leaf area index (LAI) is a key characteristic affecting a field canopy microclimate. In addition to traditional professional measuring instruments, smartphone-based methods have been used to measure forest LAI. However, when smartphone methods were used to measure conifer forest LAI, very different performances were obtained depending on whether the smartphone was held at the zenith angle or at a 57.5° angle. To further validate the potential of smartphone sensors for measuring conifer LAI and to find the limits of this method, this paper reports the results of a comparison of two smartphone methods with an LAI-2000 instrument. It is shown that the method with the smartphone oriented vertically upwards always produced better consistency in magnitude with LAI-2000. The bias of the LAI between the smartphone method and the LAI-2000 instrument was explained with regards to four aspects that can affect LAI: gap fraction; leaf projection ratio; sensor field of view (FOV); and viewing zenith angle (VZA). It was concluded that large FOV and large VZA cause the 57.5° method to overestimate the gap fraction and hence underestimate conifer LAI. For the vertically upward method, the bias caused by the overestimated gap fraction is compensated for by an underestimated leaf projection ratio.