The performance of Mobile Broadband (MBB) services of Fourth Generation (4G) and Third Generation (3G) mobile networks over urban morphology is studied in Malaysia based on experimental measurements of drive test data. The aim of this study is to provide a roadmap for service providers to establish a realistic plan for future Fifth Generation (5G) networks. This work is a continuation of our previous work for the scope of rural areas in Malaysia. The MBB measurement data have been gathered through drive tests conducted in the urban areas of four states throughout Malaysia (namely, Klang Valley/Selangor, Johor, Sarawak and Sabah) to characterise and analyse MBB performances. The gathered data are from the cities, highways and federal roads of the chosen states, and encompasses three main Mobile Network Operators (MNOs). Data has been collected in a time span of 2 months, from January to February, using the Samsung Galaxy S6 smartphone handsets. Four MBB Key Performance Indicators (KPIs) are considered in this study (coverage, latency, satisfaction and speed) for two MBB services (web browsing and video streaming). The measurement data for characterising the performance of each MBB service has been collected using a dedicated smartphone handset. YouTube videos with 720p and 1080p resolutions have been sequentially streamed to assess the performance of MBB video-streaming services. Three distinct websites (Google, Instagram and mStar) have been accessed to evaluate the performance of MBB web-browsing services. The experimental methodology of this study integrates several diversified elements including four different urban states, four distinct KPIs, three main MNOs, two MBB services and two radio networks (4G and 3G), which are both accessible by the smartphones when available to mimic real-world scenarios. The results of this study reveal that the performance of 4G radio networks is generally superior to that of 3G. For instance, 4G networks achieved a vMOS score of more than 3 for both MBB video-streaming and web-browsing services, while 3G networks scored less than 3 across all four study areas. The analysed experimental results confirmed that compared to 3G networks, 4G technology presents an enhancement factor of up to 1.6 and 4.2 in download speed when streaming a video and browsing a web page, respectively. The study outcomes can contribute to the efficient planning of non-standalone (NSA) 5G networks in Malaysia where 5G networks will be aided by existing 4G infrastructures. Analysing the 4G coverage performance is the first step towards deciding the deployment rate of NSA 5G in Malaysia.