Ever-increasing hardware capabilities and computation powers have enabled acquisition and analysis of big scientific data at the nanoscale routine,though much of the data acquired often tu out to be redundant,noisy and/or irrelevant to the problems of interest,and it remains nontrivial to draw clear mechanistic insights from pure data analy tics.In this work,we use scanning probe microscopy (SPM) as an example to demonstrate deep data methodology for nanosciences,transitioning from brute-force analytics such as data mining,correlation analysis and unsupervised classification to informed and/or targeted causative data analttics built on sound physical understanding.Three key ingredients of such deep data analttics are presented.A sequential excitation scanning probe microscopy (SE-SPM) technique is first developed to acquire high-quality,efficient and physically relevant data,which can be easily implemented on any standard atomic force microscope (AFM).Brute-force physical analysis is then carried out using a simple harmonic oscillator (SHO) model,enabling us to derive intrinsic electromechanical coupling of interest.Finally,principal component analysis (PCA) is carried out,which not only speeds up the analysis by four orders of magnitude,but also allows a clear physical interpretation of its modes in combination with SHO analysis.A rough piezoelectric material has been probed using such a strategy,enabling us to map its intrinsic electromechanical properties at the nanoscale with high fidelity,where conventional methods fail.The SE in combination with deep data methodology can be easily adapted for other SPM techniques to probe a wide range of functional phenomena at the nanoscale.