Aroma is a key quality attribute of apples, making major contributions to commercial value and consumer choice. However, the mechanism underlying molecular regulation of aroma formation genes and transcription factors remains poorly understood in apples. Here, we investigated the aroma volatile profiles of two apple varieties with distinctive flavors using headspace solid-phase microextraction (HS-SPME) combined with gas chromatography-mass spectrometry (GC-MS). A total of 35 volatile compounds were identified in Granny Smith and Jonagold apples. Aldehydes were the most abundant volatiles contributing to the aroma in Granny Smith apple while esters were the dominant volatile compounds in Jonagold apple. In order to know more about the expression levels of aroma-related genes involved in the metabolic pathways, transcriptome sequencing of these two different apple varieties was conducted utilizing the Illumina platform. In total, 94 differentially expressed genes (DEGs) were found in the fatty acid metabolism, amino acid metabolism, the mevalonate pathway and phenylpropanoid pathway. Furthermore, compared to the Granny Smith apple, the expression of multiple genes and transcription factors were upregulated in the Jonagold apple, which might play important roles in the synthesis of aroma volatile compounds. Our study contributes toward better understanding on the molecular mechanism of aroma synthesis in apples and provides a valuable reference for metabolic engineering and flavor improvement in the future.