As the land ecosystem provides the necessary basic material resources for human development, land ecological security (LES) plays an increasingly important role in sustainable development. Given the degradation of land ecological security under rapid urbanization and the urgent LES requirements of urban populations, a comprehensive evaluation method, named Double Land Ecological Security (DLES), has been introduced with the city of Guangzhou, China, as a case study, which evaluates the LES in regional and unit scales for reasonable and specific urban planning. In the evaluation process with this method, we have combined the material security with the spiritual security that is inevitably associated with LES. Some new coefficients of land-security supply/demand distribution and technology contribution for LES evaluation have also been introduced for different spatial scales, including the regional and the unit scales. The results for Guangzhou indicated that, temporally, the LES supply indices were 0.77, 0.84 and 0.77 in 2000, 2006 and 2009 respectively, while LES demand indices for the city increased in 2000, 2006 and 2009 from 0.57 to 0.95, which made the LES level decreased slowly in this period. Spatially, at the regional scale, the urban land ecological security (ULES) level decreased from 0.2 (marginal security) to -0.18 (marginal insecurity) as a whole; in unit scale, areas in the north and in parts of the east were relatively secure and the security area was shrinking with time, but the central and southern areas turned to be marginal insecurity, especially in 2006 and 2009. This study proposes that DLES evaluation should be conducted for targeted and efficient urban planning and management, which can reflect the LES level of study area in general and in detail.