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Canopy closure (CC), a useful biophysical parameter for forest structure, is an important indicator of forest resource and biodiversity. Light Detection and Ranging (LiDAR) data has been widely studied recently for forest ecosystems to obtain the three-dimensional (3D) structure of the forests. The components of the Unmanned Aerial Vehicle LiDAR (UAV-LiDAR) are similar to those of the airborne LiDAR, but with higher pulse density, which reveals more detailed vertical structures. Hemispherical photography (HP) had proven to be an effective method for estimating CC, but it was still time-consuming and limited in large forests. Thus, we used UAV-LiDAR data with a canopy-height-model-based (CHM-based) method and a synthetic-hemispherical-photography-based (SHP-based) method to extract CC from a pure poplar plantation in this study. The performance of the CC extraction methods based on an angular viewpoint was validated by the results of HP. The results showed that the CHM-based method had a high accuracy in a 45° zenith angle range with a 0.5 m pixel size and a larger radius (i.e., <i>k</i> = 2; <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mrow><msup><mi>R</mi><mn>2</mn></msup></mrow></semantics></math></inline-formula> = 0.751, <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mrow><mi>R</mi><mi>M</mi><mi>S</mi><mi>E</mi></mrow></semantics></math></inline-formula> = 0.053), and the accuracy declined rapidly in zenith angles of 60° and 75° (<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mrow><msup><mi>R</mi><mn>2</mn></msup></mrow></semantics></math></inline-formula> = 0.707, 0.490; <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mrow><mi>R</mi><mi>M</mi><mi>S</mi><mi>E</mi></mrow></semantics></math></inline-formula> = 0.053, 0.066). In addition, the CHM-based method showed an underestimate for leaf-off deciduous trees with low CC. The SHP-based method also had a high accuracy in a 45° zenith angle range, and its accuracy was stable in three zenith angle ranges (<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mrow><msup><mi>R</mi><mn>2</mn></msup></mrow></semantics></math></inline-formula>: 0.688, 0.674, 0.601 and <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mrow><mi>R</mi><mi>M</mi><mi>S</mi><mi>E</mi></mrow></semantics></math></inline-formula> = 0.059, 0.056, 0.058 for a 45°, 60° and 75° zenith angle range, respectively). There was a similar trend of CC change in HP and SHP results with the zenith angle range increase, but there was no significant change with the zenith angle range increase in the CHM-based method, which revealed that it was insensitive to the changes of angular CC compared to the SHP-based method. However, the accuracy of both methods showed differences in plantations with different ages, which had a slight underestimate for 8-year-old plantations and an overestimate for plantations with 17 and 20 years. Our research provided a reference for CC estimation from a point-based angular viewpoint and for monitoring the understory light conditions of plantations.