China announced its national goal to reach the peak of carbon emission by 2030 and achieve carbon neutrality by 2060, during the General Assembly of the United Nations in September 2020. In this context, enhancing the terrestrial ecosystem carbon sink (referred to as terrestrial C sink) is an important way to slow down the continuous increase in atmospheric carbon dioxide (CO₂) concentration and to achieve C neutrality target. China's Loess Plateau is both the largest and deepest loess deposit in the world, and it is the initiative of "One Belt and One Road" construction and the natural ecological barrier in the west of China. Indigenous vegetation of the plateau has suffered damage because of growing food needs since the early 1990s. Then, numerous soil erosion control and vegetation restoration projects have been put into practice. With the implementation of the Grain-for-Green Project and vegetation construction in 1999, the Loess Plateau has become the most successful ecological restoration zone. For example, soil organic C sequestration has greatly increased in recent years, specially, remote sensing images indicated that the vegetation coverage on the Loess Plateau increased from 32% in 1999 to 71% in 2020. With increasing scientific and political interest in regional aspects of the global C cycle, there is a strong impetus to better understand the C storage of terrestrial ecosystems of the Loess Plateau. Based on the policy of the "High-quality Development of the Yellow River" and "Dual Carbon Strategic Goals", the C sequestration effect of the Loess Plateau will face a major turning point and severe challenge. By this way, this article reviewed the significance and countermeasures of vegetation construction on the Loess Plateau to carbon neutrality. Here, we firstly reviewed the background and process of vegetation construction on the Loess Plateau, and then summarized the C sequestration effect in the process of vegetation construction. According to the C fixation and discharge process, we put forward a series of measures and countermeasures to reduce C emissions, including optimizing the management pattern of vegetation construction, strengthening the top-level design of science and technology, enhancing the C sink capacity of vegetation construction, and building up the C trading market for returning farmland to forest/grass, improving the statistical monitoring system and C calculation standard, etc. Looking forward, the possible problems and challenges in the later stage of vegetation construction were prospected, which would provide importantly scientific and technological support for realizing the strategic goal of C neutrality in our country.